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He was born in Himara,[1]Northern Epirus, in modern southern Albania, then part of the Ottoman Empire. In 1810 he went to Naples in Italy, where he remained until 1819, studying military theory and learning Latin and French. In 1819, he returned to his homeland to prepare a geographic survey for his school, but was arrested by Ali Pasha, the ruler of Ioannina, who employed him at his court as a military adviser.

In August 1824, after Ali’s death, together with his brothers Nikolaos and Zachos Milios, Spyromilios, he travelled south and joined the ongoing Greek War of Independence. In August 1825 he was fighting in the Third Siege of Missolonghi, at the head of a group of 250 armed Himariotes. Named General in September, he was sent as a member of a commission to Nafplion in January 1826, to ask the government for more effective aid to the besieged city. Little was achieved, and although Spyromilios tried to arrange for a British ship to evacuate the garrison, it was too late. Spyromilios was thus forced to remain a spectator of the garrison's disastrous attempt to sally and break through the Ottoman lines, during which his brother Nikolaos was killed.

After the end of the War of Independence, Spyromilios settled in Thebes, but as a known supporter of Kapodistrias, he was imprisoned for 9 months in the Palamidi fortress (September 1833-June 1834). Released and reinstated to the army, he became director of the Evelpidon Military Academy in 1840-1844. The first Greek to hold that post, he also wrote the Academy's first book of regulations. From this position he participated in the 3 September 1843 Revolution that led to the granting of the first Constitution of Greece. This led him to be considered as an enemy of King Otto, but he soon regained the King's trust. He was appointed General Secretary of the Ministry of Military Affairs in 1848 and adjutant to the King, and in 1850 he was appointed Minister of Military Affairs, a post he kept until 1853. Following the outbreak of the Crimean War, he supported Greek revolts in the Ottoman Empire, despite the neutrality forced upon Greece by Britain and France. His involvement in a revolt in Epirus (1854) led to his dismissal from his offices and his suspension from the Army.

Retired from the Army, he returned to politics from 1859, and served as Minister of Military Affairs in the several cabinets:

^Ivo Banac, John G. Ackerman, Roman Szporluk, Wayne S. Vucinich (1981). Nation and ideology: essays in honor of Wayne S. Vucinich. East European Monographs. p. 46. ISBN978-0-914710-89-9. Cheimarriote veterans played a significant role in the Greek War of Independence, 1821-1830. Among those who became officers in the Greek insurrectionary forces were: ... The most notable of these officers was General Spyromelios."

Land and Revolution in Modern Greece, 1800-1881: The Transition in the Tenure and Exploitation of Land from Ottoman Rule to Independence. William W. McGrew. Kent State University Press, 1985. ISBN 0-87338-316-8.